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First-Principles Studies of Contact Effects on Transport Properties of Metal-Molecule Junctions

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Date: 07-13-2006
Start Time: 11:00am
End Time: 12:00pm
Speaker: Jeffrey B. Neaton
From: The Molecular Foundry, LBNL
Location: 414 Schapiro/CEPSR
Hosted by: Center for Integrated Science

Abstract:

I will describe two separate theoretical studies of the role played by metallic contacts in determining the low-bias transport properties of metal-molecule junctions. Recent break-junction experiments have reported the conductance of H2 molecular junctions drops by more than a factor of two when Pt contacts were simply replaced with Pd. We are able to explain these results surprisingly well by directly computing the conductance of H2 with Pt and Pd metallic contacts using an ab initio scattering state approach based on density functional theory. Surface polarization of the metallic electrode affects the energetic position of the frontier orbitals relative to the contact Fermi level. We study a model metal-molecule contact, benzene physisorbed on graphite. The benzene HOMO-LUMO gap, computed using the GW approximation for the electron self-energy, is substantially altered from its gas phase value, as well as differing from the results of DFT calculations. A model calculation illustrates the impact of this polarization for other conjugated molecules.

Biographical Sketch: Jeffrey B. Neaton received his Ph.D. in Physics from Cornell University in 2000, under the guidance of Neil W. Ashcroft. After a three-year stint as a departmental postdoc in the Department of Physics and Astronomy at Rutgers University, he joined the Molecular Foundry at Lawrence Berkeley National Laboratory in 2003, first as a postdoc under Steven G. Louie and eventually as permanent staff. He is presently acting lead scientist of the Foundry’s Theory group. His current research interests center on computational nanoscience, in particular the development and application of methods for calculating the structural, spectroscopic, and transport properties of inorganic and molecular nanostructures, particularly at interfaces. Present areas of interest include the electronic properties of the metal-organic interface, hybrid silicon-organic interfaces, and single-molecule junctions; self-assembly; nanoparticle superlattices; ultrathin epitaxial films of transition metal oxides, such as ferroelectrics and multiferroics; and structural and electronic phases of light elements under pressure.